A micro-mechanical model for the response of filled elastomers at finite strains

Abstract

Constitutive equations are developed for the isothermal response of particle-reinforced elastomers at finite strains. A rubbery polymer is treated as a network of chains bridged by junctions. A strand between two junctions is thought of as a series of inextensible segments linked by bonds. Two stable conformations are ascribed to a bond: flexed and extended. Deformation of a specimen induces transition of bonds from their flexed conformation to the extended conformation. A concept of trapped entanglements is adopted, according to which not all junctions are active in the stress-free state. Under straining, some entanglements are transformed from their passive (dangling) state to the active state, which results in a decrease in the average length of a strand. Stress–strain relations for an elastomer and kinetic equations for the rate of transition of bonds from their flexed conformation to the extended conformation are derived by using the laws of thermodynamics. Simple phenomenological equations are suggested for the evolution of the number of active entanglements. The model is determined by five adjustable parameters which are found by fitting experimental data in uniaxial tensile tests. Fair agreement is demonstrated between the results of numerical simulation and observations for a polysulfide elastomer reinforced with polystyrene particles and two natural rubber vulcanizates with different cross-linkers.